Dinuclear ruthenium(II) complexes [{(L)ClRuII}(2)(mu-tppz)](2+) (L = an arylazopyridine ligand) incorporating tetrakis(2-pyridyl) pyrazine (tppz) bridging ligand: synthesis, structure and spectroelectrochemical properties
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Title |
Dinuclear ruthenium(II) complexes [{(L)ClRuII}(2)(mu-tppz)](2+) (L = an arylazopyridine ligand) incorporating tetrakis(2-pyridyl) pyrazine (tppz) bridging ligand: synthesis, structure and spectroelectrochemical properties
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Creator |
CHANDA, N
LAYE, RH CHAKRABORTY, S PAUL, RL JEFFREY, JC WARD, MD LAHIRI, GK |
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Subject |
mixed-valence chemistry
creutz-taube ion electron-transfer crystal-structure electrochemical properties spectroscopic properties binuclear complexes ancillary ligands metal-complexes molecular wires |
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Description |
A series of dinuclear complexes [{(L1-4)C1Ru(II)}(2) (mu-tppz)][ClO4](2) {[1](ClO4)(2) to [4](ClO4)(2)} has been prepared, in which two {Ru-II(L1-4)Cl}(+) fragments [L = a 2-arylazopyridine ligand of the type 2-(C5H4N)-N=N-C6H4R; for L-1, R = H; L-2, R = p-Me; L-3, R = p-Cl; L-4, R = m-Me] are linked by the bridging ligand tppz [2,3,5,6-tetrakis(2-pyridyl) pyrazine]. A single isomer forms during the synthesis in each case, and the crystal structure of [4](ClO4)(2) shows it to be a twofold-symmetric isomer with each ligand L arranged such that its pyridine donor is on the long axis of the molecule (trans to the pyrazine ring of tppz) and the azo donor is trans to one of the pyridyl donors of tppz. This allows the peripheral aryl ring attached to the azo unit of each ligand L to be oriented over either face of the bridging ligand giving a three-layer pi-stacked (aryl-pyrazine-aryl) sandwich. Electrochemical studies revealed (i) separations of 190-250 mV (depending on the aryl substituent of L) between the successive Ru(II)/ Ru(III) couples, indicative of a significant inter-metallic electronic coupling, and (ii) several ligand-based reductions of the pi-acceptor pyrazine and arylazopyridine ligands. A UV/Vis/NIR spectroelectrochemical study showed the presence of an IVCT transition at ca. 1900 nm in MeCN for the Ru(II)-Ru(III) mixed-valence states, whose narrowness is indicative of borderline class III behaviour. Several reduced forms of the complexes were also spectroscopically characterised.
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Publisher |
ROYAL SOC CHEMISTRY
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Date |
2011-08-28T10:21:15Z
2011-12-26T12:58:00Z 2011-12-27T05:46:45Z 2011-08-28T10:21:15Z 2011-12-26T12:58:00Z 2011-12-27T05:46:45Z 2002 |
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Type |
Article
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Identifier |
JOURNAL OF THE CHEMICAL SOCIETY-DALTON TRANSACTIONS, (18), 3496-3504
1472-7773 http://dx.doi.org/10.1039/b204862k http://dspace.library.iitb.ac.in/xmlui/handle/10054/11714 http://hdl.handle.net/10054/11714 |
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Language |
en
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